Silk-fibroin based biomaterials have been utilized for applications in biomedical and biotechnological fields. Several techniques for processing silk-fibroin have been developed, such as electrospinning, sonication, and chemical modification. Often, these processes yield silk biomaterials that are formed and/or stabilized through β-sheet assembly, with the size and distribution of the crystalline β-sheet regions regulating the mechanical properties and degradation rates of the silk biomaterials. See Jin H. J. et al., 3 Biomacromolecules 1233 (2002); Wang X. et al., 29 Biomaterials 1054 (2008); Murphy A. R. et al., 29 Biomaterials 2829 (2008); and Wang Y. et al., 29 Biomaterials 3415 (2008). Nevertheless, there remains a need for silk-based materials that present different characteristics, based on different mechanisms that can be used for various applications in the biomedical arena.